Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion for efficient oxygen evolution reaction

doi:10.1007/s11705-021-2087-1

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (7) : 1114-1124 https://doi.org/10.1007/s11705-021-2087-1

RESEARCH ARTICLE

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion for efficient oxygen evolution reaction

Lingtao Kong, Zhouxun Li, Hui Zhang, Mengmeng Zhang, Jiaxing Zhu, Mingli Deng(

), Zhenxia Chen, Yun Ling, Yaming Zhou

Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, China

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Abstract

Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal–organic–frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni²⁺ and Fe³⁺. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO₂. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm^–2 and a small Tafel slope of 84.4 mV·dec^–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

Keywords metal–organic framework pyrolysis ultrafine Fe-modulated Ni nanoparticles oxygen evolution reaction

Corresponding Author(s): Mingli Deng

Online First Date: 29 September 2021 Issue Date: 15 July 2022

Cite this article:

Lingtao Kong,Zhouxun Li,Hui Zhang, et al. Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion for efficient oxygen evolution reaction[J]. Front. Chem. Sci. Eng., 2022, 16(7): 1114-1124.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2087-1
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I7/1114

Scheme 1 Schematic illustration of the synthetic strategy for the Fe-modulated Ni NPs.

Fig.1 (a) PXRD patterns of the produced samples; (b) IR spectra of (1) UiO-bpydc, (2) NiUiO-bpydc, (3) Ni₁Fe₁UiO-bpydc and (4) FeUiO-bpydc; (c) TGA profile of Ni₁Fe₁UiO-bpydc under nitrogen; (d) PXRD patterns of (1) Ni₁Fe₁UiO-bpydc-500, (2) Ni₁Fe₁UiO-bpydc-600 and (3) Ni₁Fe₁UiO-bpydc-700 (Green: PDF#87-0712, Metallic Ni; Purple: PDF#50-1089, ZrO₂).

Fig.2 HRTEM images of (a) Ni₁Fe₁UiO-bpydc-500, (b) Ni₁Fe₁UiO-bpydc-600, (c) Ni₁Fe₁UiO-bpydc-700, (d) HAADF images for Ni₁Fe₁UiO-bpydc-500, (e) Ni₁Fe₁UiO-bpydc-600 and (f) Ni₁Fe₁UiO-bpydc-700, and the corresponding EDX mapping images of N, Zr, Ni and Fe elements.

Fig.3 XPS spectra of Ni₁Fe₁UiO-bpydc-500(1), Ni₁Fe₁UiO-bpydc-600(2) and Ni₁Fe₁UiO-bpydc-700(3). (a) Full spectra; (b) high-resolution C 1s XPS spectra; (c) high-resolution N 1s XPS spectra; (d) high-resolution Ni 2p XPS spectra; (e) high-resolution Fe 2p XPS spectra; (f) high-resolution Zr 3d XPS spectra.

Tab.1 Elemental composition results of samples by ICP-AES analysis.

Fig.4 (a) Raman spectra of Ni₁Fe₁UiO-bpydc-500, Ni₁Fe₁UiO-bpydc-600 and Ni₁Fe₁UiO-bpydc-700; (b) N₂ adsorption-desorption isotherms of the as-made samples.

Tab.2 Texture parameters of these as-made samples

Fig.5 Electrochemical OER activity of as-made samples in 1 mol·L^–1 KOH solution: (a) polarization curves; (b) the corresponding Tafel plots derived from the polarization curves; (c) the relationship between scan rate and the current density; (d) Nyquist plots of the corresponding samples, the inset shows the equivalent circuit employed to fit the experimental data; (e) chronopotentiometric test curves of IrO₂ and Ni₁Fe₁UiO-bpydc-600 measured at 10 mA·cm^–2; (f) linear sweep voltammetry (LSV) curves of Ni₁Fe₁UiO-bpydc-600 before and after 4000 cyclic voltammetry (CV) cycles with the scan rate of 20 mV·s^–1.

Fig.6 Electrochemical OER activities of the corresponding samples in 1 mol·L^–1 KOH solution: (a) polarization curves; (b) the overpotential and Tafel slope derived from the polarization curves.

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